CN107427770B - Catalytic ceramic candle filter and method for cleaning process exhaust or exhaust gas - Google Patents

Catalytic ceramic candle filter and method for cleaning process exhaust or exhaust gas Download PDF

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Publication number
CN107427770B
CN107427770B CN201580077975.7A CN201580077975A CN107427770B CN 107427770 B CN107427770 B CN 107427770B CN 201580077975 A CN201580077975 A CN 201580077975A CN 107427770 B CN107427770 B CN 107427770B
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filter
palladium
exhaust gas
exhaust
wall
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CN107427770A (en
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F·卡斯特利诺
L·S·佩德森
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Topsoe AS
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Haldor Topsoe AS
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    • B01J23/64—Platinum group metals with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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    • B01J23/6482—Vanadium
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    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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    • B01D53/8643—Removing mixtures of carbon monoxide or hydrocarbons and nitrogen oxides
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    • B01D2258/00—Sources of waste gases
    • B01D2258/01—Engine exhaust gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0233—Other waste gases from cement factories
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases
    • B01D2258/0291—Flue gases from waste incineration plants
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2250/00—Combinations of different methods of purification
    • F01N2250/12—Combinations of different methods of purification absorption or adsorption, and catalytic conversion
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2370/00—Selection of materials for exhaust purification
    • F01N2370/02—Selection of materials for exhaust purification used in catalytic reactors
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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    • F01N2510/00—Surface coverings
    • F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
    • F01N2510/068—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings
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Abstract

The present invention relates to a ceramic candle filter and the use of said filter for the removal of particulate matter in the form of soot, ash, metals and metal compounds, as well as hydrocarbons and nitrogen oxides, present in process exhaust gas or engine exhaust gas, the filter comprising a combined SCR and oxidation catalyst arranged in the dispersion side and/or in the walls of the filter; and a palladium-containing catalyst arranged on the permeate side of the filter and located in the wall of the filter facing the permeate side.

Description

Catalyzed ceramic candle filter and method for cleaning process exhaust or gas
The present invention relates to ceramic candle filters and methods for cleaning process off-gas or exhaust gas. More particularly, the present invention provides a catalyzed ceramic candle filter for removing dust and particulate matter from process exhaust or engine exhaust gases, as well as harmful components contained in these gases. Catalyzed ceramic candle filters are particularly useful for cleaning process or feed gases from industrial processes involving combustion (e.g., production of minerals, glass, cement, waste incineration) or from coal-fired boilers and engines.
Ceramic filters in the form of filter candles are used in many industries to remove particulate matter from process gases. They are one of the most efficient types of dust collectors available and can achieve collection efficiencies for particulate matter of greater than 99%. The filter may be made from a variety of ceramic materials, including ceramic fibers made from alkali and alkaline earth metal silicates or aluminosilicates.
The high particulate removal efficiency of ceramic candle filters is due in part to the dust cake formed on the surface of the candle filter and in part to the composition and porosity of the candle filter. In order to provide sufficient filtration activity and an acceptably low pressure drop across the filter, conventional ceramic candle filters have a porosity of 70-90%. The wall thickness of these filters should be in the range of 10-20mm to obtain sufficient stability and mechanical strength.
Particle-containing process gases often contain a variety of contaminants, such as NOxVolatile Organic Compounds (VOC), SO2、CO、NH3Two, two
Figure BDA0001411816220000011
And dioxins and furans, the concentration of which must be reduced according to local regulations. For this purpose, several conventional methods can be used.
Can effectively reduce gas pollutants such as NOx, VOC and II by contacting with a catalyst
Figure BDA0001411816220000012
And furan. In particular, catalysts based on vanadium oxides are the catalysts commonly used for the passage of NOx with NH3To reduce NOx in static and automotive applications.
The catalyst is oxidized and reacted with NH in combination3The SCR reaction of (a) is active in both hydrocarbon (VOC) and NOx removal.
Vanadium oxides are also known as active oxidation catalysts. Vanadium oxide catalysts in CO in contrast to noble metal catalysts (e.g., Pd catalysts)2The selectivity in formation is low and a certain amount of CO is produced during the oxidation reaction. CO cannot be oxidized to carbon dioxide at a viable reaction rate by contact with a vanadium oxide catalyst, but rather requires the presence of a noble metal catalyst, such as palladium.
We have found that when very small amounts of palladium are provided on the inner surface, i.e. the permeate side or the wall portion facing the permeate side of a vanadium oxide catalysed candle filter, a lower evolution of ammonia and carbon monoxide from the filter results.
In accordance with this discovery, the present invention provides a ceramic candle filter suitable for use in the removal of particulate matter in the form of soot, ash, metals and metal compounds, as well as hydrocarbons and nitrogen oxides, present in process exhaust or engine exhaust gases, the filter comprising a combined SCR and oxidation catalyst disposed on the dispersion side and/or within the walls of the filter; and
a palladium-containing catalyst arranged in the permeate side of the filter and/or in the wall of the filter facing the permeate side.
The terms "dispersion side" and "permeate side" as used herein refer to the flow side of the filter towards unfiltered exhaust gas and towards the flow side of filtered exhaust gas or exhaust gas, respectively.
The present invention additionally provides a process for the removal of particulate matter in the form of soot, ash, metals and metal compounds, and hydrocarbons and nitrogen oxides present in process off-gas or engine exhaust gas, which process comprises the steps of:
providing a process exhaust or engine exhaust containing a nitrogenous reductant or adding a nitrogenous reductant to an exhaust or exhaust;
passing the exhaust gas or gas through a ceramic candle filter and capturing particulate matter;
reducing the amount of soot in the particulate matter captured on the dispersion side of the filter by oxidation and reducing the amount of hydrocarbons in the exhaust gas or exhaust gas; and reducing the amount of nitrogen oxides by Selective Catalytic Reduction (SCR) of the nitrogen oxides with a nitrogenous reductant in contact with a combined SCR and oxidation catalyst disposed on the dispersion side and/or within the walls of the filter; and
the gas is passed through the walls of the filter and the amount of carbon monoxide and ammonia in the gas passing through the walls of the filter is reduced by contact with a palladium-containing catalyst arranged on the permeate side of the filter and/or in the wall of the filter facing the permeate side.
Preferably, the combined SCR and oxidation catalyst comprises vanadium oxide and titanium dioxide.
It is further preferred that the palladium-containing catalyst further comprises vanadium oxide and titanium dioxide.
The term "vanadylCompound "refers to vanadium (II) oxide (vanadium monoxide), VO; or vanadium (III) oxide (vanadium trioxide), V2O3(ii) a Or vanadium (IV) oxide (vanadium dioxide), VO2(ii) a Or vanadium (V) oxide (vanadium pentoxide), V2O5。
Preferably, the vanadium oxide used in the present invention includes vanadium (V) oxide (vanadium pentoxide) V2O5Or consist thereof.
The term "titanium dioxide" refers to titanium dioxide (TiO)2)。
The catalytically active form of palladium is palladium in metallic and/or oxidised form.
The abbreviations V/Ti and Pd/V/Ti denote a catalyst consisting of vanadium oxide and titanium oxide and a catalyst consisting of palladium, vanadium oxide and titanium oxide, respectively.
It is also preferred that the vanadium oxide/titania catalyst is additionally dispersed on the permeate side of the filter along with the palladium-containing catalyst.
Preferably, the palladium-containing catalyst contains palladium in an amount of 20 to 1000ppm per weight of filter.
These catalysts are preferred for the following reasons. The Pd/V/Ti catalyst has i) dual functions (NOx removal and VOC removal, volatile organic compounds); ii) sulfur resistance; and iii) lower SO compared to other catalyst compositions, e.g., Pt-based catalysts2And (4) oxidation activity.
For example, when a process gas containing ammonia and VOCs passes over the dispersion side of a catalyst loaded with vanadium-based oxides, NH passes over NOx3-the SCR removes ammonia from the gas before the ammonia is contacted with the permeate side. During the passage through the dispersion side, a certain amount of CO is formed after direct contact with the V/Ti catalyst due to incomplete oxidation of the VOC. By loading the Pd catalyst or Pd/V/Ti catalyst only on the permeate side and/or the walls of the filter, CO and the remaining amount of VOC are efficiently oxidized to CO2. In this way, a minimum loading of expensive palladium within the walls and/or on the permeate side of the filter can be achieved.
A further advantage is that the catalysed filter candle is sulphur resistant when using a Pd/V/Ti catalystI.e. no sulphur deactivation occurs. Pd/V/Ti catalyst also reduces SO2SO formed by oxidation3The amount of (c). If H is also present in the process gas entering the filter2S, which will also be oxidized to SO over both V/Ti and Pd/V/Ti catalysts2。
In the case of high temperature ceramic filters, various types of fibers may be used for production. These may for example consist of aluminium silicate, calcium magnesium silicate, calcium silicate fibres or mixtures thereof.
Other preferred ceramic fibers include biosoluble fibers selected from the group consisting of calcium magnesium silicates.
The catalytically active material is applied to the ceramic filter by impregnating the dispersion side and the filter wall with a slurry containing the catalytically active material (in the form of titanium dioxide particles and precursors of the active material, i.e. in the form of vanadium salts) and impregnating the permeate side with a solution of palladium salts or a slurry of titanium dioxide particles and salts of vanadium and palladium. Once impregnated, the filter is then dried and heated to the temperature required to decompose all of the catalyst precursor and activate the catalyst.
Example 1
The following example illustrates the performance obtainable with a ceramic candle filter made from calcium magnesium silicate fibres having a length of 3m and a wall thickness of 20 mm. The filter was coated in-wall with a V/Ti catalyst containing 1.26 wt% V and 2.36 wt% Ti, based on the total weight of the filter. The porosity of the coated filter was 83%. In a reactor containing 40ppm dry toluene, 19 vol.% O28% by volume of H2The filter was tested in toluene oxidation in inlet gas of O.
Toluene oxidation on V/Ti coated filters
Figure BDA0001411816220000041
As can be seen from the above table, 85% of the toluene is converted at 240 ℃. At the same temperature, the CO emission is equal to 35ppm, wet.
Example 2
The following examples illustrateThe ceramic candle filter of example 1 had the CO oxidation performance except that it was additionally coated with 36ppm Pd. With a wet CO content of about 150ppm, 19% O2And 8% of H2O gas to perform the test.
Figure BDA0001411816220000042
At 240 deg.C, 97% of the CO is oxidized to CO2。
By combining the performance of the ceramic candle filters reported in example 1 and example 2, it can be concluded that only 1ppm of CO is emitted by the candle filter catalyzed with a V/Ti catalyst on the dispersion side and a Pd/V/Ti catalyst on the permeate side.

Claims (10)

1.一种适用于除去工艺尾气或发动机废气中存在的烟灰、灰分、金属和金属化合物形式的颗粒物质以及烃和氮氧化物的陶瓷烛式过滤器，所述过滤器包括至少布置在过滤器的分散侧和/或壁内的组合的SCR和氧化催化剂，所述组合的SCR和氧化催化剂包含钒氧化物和二氧化钛；和1. A ceramic candle filter suitable for removing particulate matter in the form of soot, ash, metals and metal compounds, and hydrocarbons and nitrogen oxides present in process exhaust or engine exhaust, said filter comprising at least a filter a combined SCR and oxidation catalyst comprising vanadium oxide and titanium dioxide within the dispersing side and/or wall; and 布置在过滤器的渗透侧和过滤器朝向渗透侧的壁内的含钯催化剂。A palladium-containing catalyst is arranged in the permeate side of the filter and in the wall of the filter facing the permeate side. 2.如权利要求1所述的陶瓷烛式过滤器，其中含钯催化剂还包含钒氧化物和二氧化钛。2. The ceramic candle filter of claim 1, wherein the palladium-containing catalyst further comprises vanadium oxide and titanium dioxide. 3.如权利要求1或2所述的陶瓷烛式过滤器，其中含钯催化剂含有量为20至1000ppm/过滤器重量的钯。3. The ceramic candle filter of claim 1 or 2, wherein the palladium-containing catalyst contains palladium in an amount of 20 to 1000 ppm per filter weight. 4.如权利要求1所述的陶瓷烛式过滤器，其中过滤器的陶瓷材料选自硅铝酸盐、硅酸钙镁、硅酸钙纤维或其混合物。4. The ceramic candle filter of claim 1, wherein the ceramic material of the filter is selected from the group consisting of aluminosilicates, calcium magnesium silicates, calcium silicate fibers, or mixtures thereof. 5.如权利要求4所述的陶瓷烛式过滤器，其中过滤器的陶瓷材料由选自硅酸钙镁的生物可溶性纤维组成。5. The ceramic candle filter of claim 4, wherein the ceramic material of the filter consists of biosoluble fibers selected from calcium magnesium silicates. 6.一种用于除去工艺尾气或发动机废气中存在的烟灰、灰分、金属和金属化合物形式的颗粒物质以及烃和氮氧化物的方法，所述方法包括以下步骤：6. A method for removing particulate matter in the form of soot, ash, metals and metal compounds, and hydrocarbons and nitrogen oxides present in process exhaust or engine exhaust, said method comprising the steps of: 提供含有含氮还原剂的工艺尾气或发动机废气或添加含氮还原剂至工艺尾气或废气；Provide process exhaust gas or engine exhaust gas containing nitrogenous reducing agent or add nitrogenous reducing agent to process exhaust gas or exhaust gas; 将尾气或废气通过陶瓷烛式过滤器，并在过滤器的分散侧上捕获颗粒物质；Pass exhaust or exhaust gas through a ceramic candle filter and capture particulate matter on the dispersing side of the filter; 通过氧化减少在过滤器的分散侧上捕获的颗粒物质中的烟灰量，并减少尾气或废气中的烃的量，以及通过氮氧化物与含氮还原剂的选择性催化还原(SCR)来减少氮氧化物的量，所述含氮还原剂与布置在过滤器的分散侧和/或壁内的组合的SCR和氧化催化剂接触，所述组合的SCR和氧化催化剂包含钒氧化物和二氧化钛；和Reduction of the amount of soot in particulate matter captured on the dispersing side of the filter by oxidation, and reduction of the amount of hydrocarbons in the exhaust or exhaust gas, and by selective catalytic reduction (SCR) of nitrogen oxides with nitrogenous reductants the amount of nitrogen oxides that the nitrogenous reductant is contacted with a combined SCR and oxidation catalyst comprising vanadium oxide and titanium dioxide disposed within the dispersing side and/or wall of the filter; and 使气体通过过滤器的壁，并且通过与含钯催化剂接触而减少通过过滤器壁的气体中的一氧化碳和氨的量，所述含钯催化剂布置在过滤器的渗透侧和/或过滤器朝向渗透侧的壁内。Passing the gas through the wall of the filter and reducing the amount of carbon monoxide and ammonia in the gas passing through the wall of the filter by contact with a palladium-containing catalyst disposed on the permeate side of the filter and/or towards the permeate inside the side wall. 7.如权利要求6所述的方法，其中含钯催化剂还包含钒氧化物和二氧化钛。7. The method of claim 6, wherein the palladium-containing catalyst further comprises vanadium oxide and titanium dioxide. 8.如权利要求6或7所述的方法，其中含钯催化剂含有量为20至1000ppm/过滤器重量的钯。8. The method of claim 6 or 7, wherein the palladium-containing catalyst contains palladium in an amount of 20 to 1000 ppm per filter weight. 9.如权利要求6所述的方法，其中过滤器的陶瓷材料选自硅铝酸盐、硅酸钙镁、硅酸钙纤维或其混合物。9. The method of claim 6, wherein the ceramic material of the filter is selected from the group consisting of aluminosilicates, calcium magnesium silicates, calcium silicate fibers, or mixtures thereof. 10.如权利要求6所述的方法，其中过滤器的陶瓷材料包括选自硅酸钙镁的生物可溶性纤维。10. The method of claim 6, wherein the ceramic material of the filter comprises biosoluble fibers selected from the group consisting of calcium magnesium silicates.
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